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A bioactive micro/nanostructured calcium phytate coating was successfully prepared on titanium surfaces by chemical conversion deposition, mainly through hydrothermal treatment of a mixed solution of phytic acid and saturated calcium hydroxide solution. Ultraviolet radiation was carried out to improve the adhesion of the coating to the titanium substrate. Pure titanium with a sandblasted/acid-etched surface was used as the control group. The topography and chemical composition of the modified surfaces were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), and static water contact angle measurement. A pull-off test was performed to measure the coating-to-substrate adhesion strength. Bovine serum albumin was used as a model to study the protein adsorption effect. Cells were cultured on titanium surfaces for 7 days in osteogenic differentiation medium, then the osteoblast compatibility in vitro were explored by alkaline phosphatase and alizarin red staining. After 1, 2, 4 and 8 wks of immediate implantation of titanium implants into the mandibles of New Zealand white rabbits, biological effects in vivo were researched by microcomputed tomography analysis and histological evaluation. The results indicated that the roughness and hydrophilicity of the modified surfaces with micro/nanostructure remarkably increased compared to those of the control group. The pull-off test showed the average adhesion strength at the coating–substrate interface to be higher than 13.56 ± 1.71 MPa. In addition, approximately 4.41 mg/L calcium ion was released from the calcium phytate micro/nano coatings to the local environment after 48 h of immersion. More importantly, the micro/nanostructure titanium substrates significantly promoted cellular differentiation in vitro and in vivo. After 8 wks, the bone implant contact ratio (BIC, %) of the modified implants was higher than that of the control group, at 94.09 ± 0.55% and 86.18 ± 1.99% (p < 0.05). Overall, this study provided new insights into the factors promoting early osseointegration of titanium alloys, which had great potential not only for dental implants but also for various other biomaterial applications. Unlabelled Image • Micro/nanostructured coating was fabricated by chemical conversion deposition. • Titanium implant is gifted with a stable and superior hydrophilicity. • The calcium-decorated surface releases calcium ions rapidly. • Calcium phytate coating accelerates the osseointegration at an early stage. [ABSTRACT FROM AUTHOR]